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LANGMUIR · 2019 · IF 3.683

Ionic Liquid-Based Microemulsions with Reversible Microstructures Regulated by CO2

Xiaojiang Li,Baogang Wang,Shanshan Dai,Hongsheng Lu,Zhiyu Huang

CO2-responsive microemulsions based on ionic liquid 1,1,3,3-tetramethylguanidine-oleic acid (TMG-OA) have been designed to provide an approach for reducing the volatilization of amine in amine-containing microemulsions effectively and exhibit reversible transitions of microstructures. The ionic liquid TMG-OA was prepared by the direct neutralization of oleic acid (HOA) and 1,1,3,3-tetramethylguanidine (TMG, one of volatile and toxic amines). From the investigations of nuclear magnetic resonance hydrogen spectrum, pH, thermogravimetry, and automatic interface tension meter, the excellent properties of switchability, stability, and surface activity of TMG-OA were demonstrated, and then the ionic liquid-based microemulsions with CO2 response were prepared with TMG-OA (surfactant), HOA (oil phase), isopropyl alcohol (IPA, cosurfactant), and water. Interestingly, for microemulsions with a higher IPA content (47.42, 44.48 wt %), sizes of microemulsions are increased upon introducing CO2 and decreased upon addition of N2/65 °C. In addition, for microemulsions with a lower IPA content (26.22 wt %), the new microemulsions with different sizes are regenerated after the phase separation of emulsions generated by introducing CO2, and incomplete recovery of microemulsions can be observed upon addition of N2/65 °C. The reversible microstructures are induced by the swelling behavior and the reduced single phase area, which are caused by the reversible conversion between TMG-OA and HOA components.

研究领域: 化学 · 材料科学
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Science China-Chemistry · 2019 ·Vol. 62 ·期 12 ·1710-1719 · IF 6.085

Active sites in CO2 hydrogenation over confined VOx-Rh catalysts

Wang Guishuo,Luo Ran,Yang Chengsheng,Song Jimin,Xiong Chuanye,Tian Hao,Zhao Zhi-Jian,Mu Rentao,Gong Jinlong

Metal oxide-promoted Rh-based catalysts have been widely used for CO 2 hydrogenation, especially for the ethanol synthesis. However, this reaction usually suffers low CO 2 conversion and alcohols selectivity due to the formation of byproducts methane and CO. This paper describes an efficient vanadium oxide promoted Rh-based catalysts confined in mesopore MCM-41. The Rh-0.3VO x /MCM-41 catalyst shows superior conversion (~12%) and ethanol selectivity (~24%) for CO 2 hydrogenation. The promoting effect can be attributed to the synergism of high Rh dispersion by the confinement effect of MCM-41 and the formation of VO x -Rh interface sites. Experimental and theoretical results indicate the formation of til-CO at VO x -Rh interface sites is easily dissociated into *CH x , and then *CH x can be inserted by CO to form CH 3 CO*, followed by CH 3 CO* hydrogenation to ethanol.

研究领域: 催化化学 · 材料科学
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Carbon Capture Science & Technology · 2023 · IF 0

Ultrathin UiO-66-NH2 polycrystalline membrane for CO2/CH4 separation

Wufeng Wu,Jiang Fan,Dongyue Wang,Yali Zhao,Xinglei Zhao,Yanying Wei

MOF membranes exhibit impressive performance in gas separation due to their large surface area, controllable pore size and unique affinity. Here, the ultrathin UiO-66-NH 2 polycrystalline membranes with thickness of ∼320 nm are successfully prepared within 1 h using a combination of ultrasound-assisted and microwave synthesis strategies. During the reaction, high-density small MOF nuclei are produced by sodium formate ultrasound-assisted, which act as sufficient nucleation sites for heterogeneous nucleation during membrane growth, aiming for development of a continuous MOF membrane on the porous substrate. The obtained UiO-66-NH 2 membrane shows an ideal CO 2 /CH 4 selectivity of 40 due to the enhanced the interaction between CO 2 molecules and the membrane. Moreover, the narrowed pore structure further hinders the diffusion of larger-sized molecules owing to -NH 2 occupying the pore channels, resulting in elevated CO 2 /CH 4 selectivity. Compared to many other MOF membranes, the UiO-66-NH 2 polycrystalline membranes exhibit a well balance of gas permeance and CO 2 /CH 4 selectivity, which presents a new route for CO 2 capture.

研究领域: 材料科学 · 化学工程 · 环境科学
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JOURNAL OF CATALYSIS · 2024 · IF 6.5

Doping Pd2+ into NinCeOx nanofibers promotes low-temperature CO2 methanation

Mengyuan Zhang,Jian Ye,Nana Lu,Xiaoyan Lu,Kongliang Luo,Jiali Dong,Qiang Niu,Pengfei Zhang,Sheng Dai

CO 2 methanation at low temperatures is still a challenge. Herein, Ni n CeO x (n = 1–3) and Ni 2.5 Pd 0.1 CeO x nanofibers by electrospinning is reported. The main advantage of this method is to obtain the highly dispersed precursor of palladium, nickel, and cerium, overcoming the difficulty of uniform mixing in conventional preparation methods. The Ni 2.5 Pd 0.1 CeO x nanofiber catalyst exhibited outstanding catalytic performance at low temperatures (CO 2 conversion rate = 90.4 %, CH 4 selectivity = 99.6 % at 230 °C) along with exceptional stability over 300 h. EPR, Raman, and O 1s XPS confirmed that Pd 2+ doping increased oxygen vacancy concentration. In-situ infrared spectroscopy indicated that CO 2 methanation on Ni 2.5 CeO x and Ni 2.5 Pd 0.1 CeO x catalysts followed the formate pathways. Pd 2+ doping increased the number of surface oxygen vacancies and hydroxyl groups, thus increasing the amount of bicarbonates and formates. DFT calculations suggested that Pd 2+ doping increased CO 2 adsorption energy, and confirmed surface hydroxyl groups and bicarbonate being beneficial for CO 2 methanation, consequently enhancing the activity of Ni 2.5 Pd 0.1 CeO x catalyst especially at low temperatures.

CAS / MDL: 68-12-2 3375-31-3
研究领域: 材料科学 · 催化化学
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APPLIED SURFACE SCIENCE · 2020 · IF 6.182

Cu2O/Ti3C2MXene heterojunction photocatalysts for improved CO2 photocatalytic reduction performance

Junzheng Zhang,Jingjing Shi,Sheng Tao,Lei Wu,Jun Lu

Photocatalytic CO 2 reduction has been viewed as a promising approach to relieve the energy crisis and green-house effect. Cheap and high performance cocatalyst is an effective approach to enhance the photocatalytic activity . Ti 3 C 2 T x (MXene) is a new family of 2D layered materials, which can be served as an electron conductor. In this work, Cu 2 O/Ti 3 C 2 T x heterojunction composites were prepared by in situ hydrothermal growth method. Cu 2 O/Ti 3 C 2 T x with the different percentages of ultrathin Ti 3 C 2 T x (2, 5, 10, 20 and 30 mg) nanosheet in the heterostructured catalysts are noted as CuTi-X (X = 2, 5, 10, 20, 30). As prepared CuTi-10 exhibits the highest photocatalytic CO 2 reaction activity (17.55 μmol·g −1 ·h −1 for CO and 0.96 μmol·h −1 ·g −1 for CH 4 ), which is 3.1 and 4.0 times higher than that of pure Cu 2 O (5.73 μmol·g −1 ·h −1 for CO and 0.24 μmol·g −1 ·h −1 for CH 4 , respectively). The advantage of the in situ growth endows the Cu 2 O/Ti 3 C 2 T x heterojunction contact interface, which is conductive to the separation of photogenerated electrons-hole pairs. The main reason is analysed and can be attributed to that Ti 3 C 2 T x can served as an electron acceptor due to its excellent conductive properties, rendering that more photo generated electrons attend the CO 2 reduction reaction. This provides a strategy to construct the Cu 2 O/Ti 3 C 2 T x heterojunction for photocatalytic CO 2 reduction.

CAS / MDL: 6046-93-1
研究领域: 材料科学 · 环境科学 · 能源科学
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ACS Catalysis · 2020 · IF 12.35

Intermediate Adsorption States Switch to Selectively Catalyze Electrochemical CO2 Reduction

Zhangweihao Pan,Kun Wang,Kaihang Ye,Ying Wang,Hai-Yan Su,Bihua Hu,Juan Xiao,Tongwen Yu,Yi Wang,Shuqin Song

Electrochemical CO2 reduction (CO2R) powered by renewable energy to convert CO2 molecules into formate is of great interest. It is still challenging to develop an efficient CO2R catalyst with high selectivity. Herein, we adjust the adsorption states of CO2– intermediates to improve the selectivity of CO2 toward formate by doping S to Cu-based electrocatalysts. It can be found that S doping could stabilize the reductive-state Cu as the active site for CO2R. The vibration models of CO2– intermediates within in situ Raman spectroscopy reveal that the selectivity improvement is ascribed to the change of the adsorption state from coexisting O*CO– and OC*O*– to the dominating OC*O*–. The electrocatalyst manifests high selectivity and activity toward formate (maximum Faradaic efficiency as high as 76.5% and maximum partial current density 21.06 mA cm–2).

研究领域: 催化化学 · 能源材料科学
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Nanoscale · 2015 ·Vol. 8 ·期 2 ·1140-1146 · IF 7.394

CO2-switchable fluorescence of a dendritic polymer and its applications

Chunmei Gao,Shaoyu Lü,Mingzhu Liu,Can Wu,Yun Xiong

The synthesis and properties of CO2 responsive and fluorescent dendritic polymers, poly(amido amine)/Pluronic F127 (PAMAM/F127), are reported in this paper. The morphologies and sizes of PAMAM/F127 dendritic polymers were investigated by dynamic light scattering (DLS) and transmission electron microscopy (TEM). PAMAM/F127 dendritic polymers showed unimolecular micelle morphologies at low concentrations, and changed to multimolecular micelles at higher concentrations. Additionally, fluorescence spectra and confocal laser scanning microscopy images showed that PAMAM/F127 dendritic polymers exhibited a fluorescent enhancement response to the presence of CO2. Apart from that, the release behavior of PAMAM/F127 gels under simulated body fluids was investigated by choosing curcumin as the hydrophobic drug. The results indicated that PAMAM/F127 dendritic polymers can be used to improve the solubility of curcumin, and the drug released faster in the presence of CO2. Such CO2 responsive fluorescent dendritic polymers are potentially applicable in cellular imaging or drug controlled release.

CAS / MDL: 25952-53-8 6066-82-6
研究领域: 材料科学 · 生物医学工程 · 药学
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ACS Nano · 2022 · IF 18.027

ZnSe Nanorods–CsSnCl3 Perovskite Heterojunction Composite for Photocatalytic CO2 Reduction

Nuoya Li,Xujian Chen,Jin Wang,Xinmeng Liang,Lintao Ma,Xiaolang Jing,De-Li Chen,Zhengquan Li

Utilizing sunlight to convert CO2 into chemical fuels could simultaneously address the greenhouse effect and fossil fuel crisis. ZnSe nanocrystals are promising candidates for photocatalysis because of their low toxicity and excellent photoelectric properties. However, pristine ZnSe generally has low catalytic activities due to serious charge recombination and the lack of efficient catalytic sites for CO2 reduction. Herein, a ZnSe nanorods–CsSnCl3 perovskite (ZnSe–CsSnCl3) type II heterojunction composite is designed and prepared for photocatalytic CO2 reduction. The ZnSe–CsSnCl3 type II heterojunction composite exhibits enhanced photocatalytic activity for CO2 reduction with respect to pristine ZnSe nanorods. The experimental characterizations and theoretical calculations reveal that the efficient charge separation and lowered free energy of CO2 reduction facilitate the CO2 conversion on the ZnSe–CsSnCl3 heterojunction composite. This work presents a type II heterojunction composite photocatalyst based on ecofriendly metal chalcogenides and metal halide perovskites. Our study has also promoted the understanding of the CO2 reduction mechanisms on perovskite nanocrystals, which could be valuable for the development of metal halide perovskite photocatalysts.

研究领域: 材料科学 · 环境科学 · 化学
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ENVIRONMENTAL TECHNOLOGY · 2021 · IF 3.247

Influence of surfactant on CO2 adsorption of amine-functionalized MCM-41

Wenwen Huang,Jiacheng Liu,Na Rao,Guozhi Fan,Juntao Yan,Qunpeng Cheng,Guangsen Song

Concerning the increasing greenhouse effect, the development of efficient CO2 adsorbents is very important. In this study, the influence of surfactant on the adsorption performance of amine-functionalized MCM-41 was analysed. The results showed that the residual amount of surfactant in MCM-41 was gradually decreased with the increase of calcination temperature which improved the pore structure. The maximum adsorption capacity (5.495 mmol/g) appeared at PEI-MCM-41-100°C indicated that the adsorption capacity could be improved under the function of surfactant. By calculating the diffusion coefficient of CO2 adsorption process in PEI-MCM-41-100/200/300/400/550°C, the diffusion resistance of CO2 was the lowest in PEI-MCM-41-100°C, which directly proved that the synergism of surfactant and organic amine could reduce the diffusion resistance of CO2 in the pore.

研究领域: 材料科学 · 环境科学
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2021 · IF 19.503

Optimized Ni-based catalysts for methane reforming with O2-containing CO2

Guixian Deng,Guifang Zhang,Xing Zhu,Qingjie Guo,Xiangbiao Liao,Xi Chen,Kongzhai Li

Reduction of CO 2 in presence of oxidative impurity ( e.g. , O 2 ) is more promising than utilization of pure CO 2 due to skyrocketing cost for purification of captured CO 2 from air or industrial exhaust gas. In this work, Ni-based catalysts are modified by CeO 2 and ZrO 2 to suppress negative effect of O 2 on reforming of CO 2 with methane, which show high CH 4 conversion (97 %) and CO 2 conversion (95 %) at 750 °C and can maintain high CO 2 conversion even with high O 2 content. The physicochemical characterizations on fresh and spent catalysts show that the interaction among Ni, CeO 2 and ZrO 2 results in well dispersion of smaller Ni particles, even after long-term testing. In situ DRIFTS results show that Ni/CeO 2 -ZrO 2 -SiO 2 catalyst shows advantage to activate CH 4 to generate active CH 3 *, promoting the formation of CO, and the CeO 2 -ZrO 2 solid solution improves the CO 2 adsorption, thereby reducing the competitive effect of CO 2 and O 2 .

研究领域: 化学工程 · 催化材料
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CHEMICAL ENGINEERING JOURNAL · 2019 · IF 8.355

Structurally improved, urea-templated, K2CO3-based sorbent pellets for CO2 capture

Peng Wang,Jian Sun,Yafei Guo,Chuanwen Zhao,Weiling Li,Guodong Wang,Su Lei,Ping Lu

The development of K 2 CO 3 -based sorbents with desirable CO 2 capture capacity and mechanical property is highly necessary for its large-scale application. In this work, a range of extruded-spheronized K 2 CO 3 -based pellets containing different K 2 CO 3 loading (30–70 wt%) and Al 2 O 3 -based supports (i.e., activated alumina, Bayer aluminum hydroxide, kaolinite clay and calcium aluminate cement) were prepared for CO 2 capture. It is found that the distinct textural properties of different supports result in the obvious diversities in CO 2 uptake and mechanical property of K 2 CO 3 -based pellets. The activated alumina-supported sorbent pellets loaded with 50 wt% of K 2 CO 3 possess the highest CO 2 adsorption capacity of 2.29 mmol/g. It is mainly attributed to the moderate amounts of active component contributing to good textural properties and abundant CO 2 -philic sites, whereas excessive K 2 CO 3 loading will cause the destruction of porous structure, consequently the inferior CO 2 uptake. Moreover, the addition of 15 wt% of urea can furher enhace CO 2 uptake of the activated alumina-supported sorbent pellets loaded with 50 wt% of K 2 CO 3 , ∼3.10 mmol CO 2 /g. The improved CO 2 uptake is due to the significantly enhanced porosity of sorbent pellets as a result of urea decomposition. In addition, the urea-templated sorbent pellets still maintain the high compressive strength (18.96 MPa) and good attrition resistance (a weight loss of 0.59% after 4000 rotations).

CAS / MDL: 584-08-7
研究领域: 材料科学 · 环境科学
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Journal of Environmental Chemical Engineering · 2021 · IF 5.909

MOFs-derived C-In2O3/g-C3N4 heterojunction for enhanced photoreduction CO2

Mengyang Xu,Xiaoxue Zhao,Haopeng Jiang,Songtao Chen,Pengwei Huo

Converting carbon dioxide into valuable chemicals is seen as a promising strategy for slowing global warming while enriching energy supplies. Photocatalysts derived from Metal-Organic Frameworks (MOFs) can not only overcome the problem of poor stability of MOFs, but also inherit the advantages of MOFs to some extent. Herein, carbon doped In 2 O 3 (C-In 2 O 3 ) hollow tubular is synthesized by calcination of MIL-68(In) as sacrificial template. Then C-In 2 O 3 and g-C 3 N 4 are hydrothermal to obtain C-In 2 O 3 /g-C 3 N 4 heterojunction . The unique hollow tubular structure, carbon doping and type-II heterojunction of C-In 2 O 3 /g-C 3 N 4 expand the light absorption capacity and promote the separation of photogenerated electron-hole pairs, thus significantly improve the activity of photocatalytic reduction of CO 2 . Among them, C-In 2 O 3 /g-C 3 N 4 -5 shows the highest CO 2 reduction activity towards CO (153.42 μmol/g/h) and CH 4 (110.31 μmol/g/h).

CAS / MDL: 207398-97-8
研究领域: 材料科学 · 环境科学
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